Performance and mechanism of sulfamethoxazole degradation on a Magnéli-phase Ti(4)O(7) reactive electrochemical membrane

Magnéli相Ti(4)O(7)反应电化学膜上磺胺甲噁唑降解的性能和机理

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Abstract

Antibiotics have emerged as a new class of environmental contaminants of global concern due to their persistence and potential ecotoxicological impacts. In order to enhance antibiotic removal efficiency, it is necessary to develop cost-effective and environmentally friendly wastewater treatment technologies. Magnéli-phase titanium oxide (Ti(4)O(7)) presents a promising solution, combining excellent metallic-like conductivity with ceramic-like corrosion resistance. In this study, the electrochemical oxidation of sulfamethoxazole (SMX) with a Ti(4)O(7) reactive electrochemical membrane (REM) as the anode and stainless steel as the cathode was systematically investigated. The effects of key operational parameters, including current density, initial pH, supporting electrolyte type and concentration, and the presence of humic acid (HA) on SMX degradation were evaluated. Under optimal conditions (current density of 0.08 mA cm(-2), pH of 7, supporting electrolyte of 0.1 mol L(-1) Na(2)SO(4), no HA effect, and pump circulation), 99.7% SMX degradation was achieved within 2 hours. Quenching experiments and electron paramagnetic resonance (EPR) analysis confirmed that hydroxyl radicals (˙OH) played a dominant role in SMX degradation. High-performance liquid chromatography coupled with quadrupole time-of-flight tandem mass spectrometry (HPLC-Q-TOF-MS/MS) identified key degradation intermediates, revealing three primary SMX degradation pathways: (1) ˙OH-mediated amino group oxidation, (2) S-N bond cleavage, and (3) -NH(2) hydroxylation. Additionally, Ecological Structure Activity Relationships (ECOSAR) software analysis demonstrated a significant reduction in overall toxicity following Ti(4)O(7) oxidation. In summary, the Ti(4)O(7) REM exhibits exceptional oxidation efficiency with low energy consumption, demonstrating strong practical feasibility and promising application potential for antibiotic-contaminated wastewater treatment.

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